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Unraveling and Mitigating the Storage Instability of Fluoroethylene Carbonate-Containing LiPF6 Electrolytes To Stabilize Lithium Metal Anodes for High-Temperature Rechargeable Batteries
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England.ORCID iD: 0000-0002-5342-3686
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-2004-5869
Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
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2019 (English)In: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, no 7, p. 4925-4935Article in journal (Refereed) Published
Abstract [en]

Implementing Li metal anodes provides the potential of substantially boosting the energy density of current Li-ion battery technology. However, it suffers greatly from fast performance fading largely due to substantial volume change during cycling and the poor stability of the solid electrolyte interphase (SEI). Fluoroethylene carbonate (FEC) is widely acknowledged as an effective electrolyte additive for improving the cycling performance of batteries consisting of electrode materials that undergo large volume changes during cycling such as Li metal. In this study, we report that while FEC can form a robust SEI on the electrode, it also deteriorates the shelf life of electrolytes containing LiPF6. The degradation mechanism of LiPF6 in FEC solutions is unraveled by liquid-and solid-state NMR. Specifically, traces of water residues induce the hydrolysis of LiPF6, releasing HF and PF5 which further trigger ring-opening of FEC and its subsequent polymerization. These reactions are significantly accelerated at elevated temperatures leading to the formation of a three-dimensional fluorinated solid polymer network. Moisture scavenger additives, such as lithium 4,5-dicyano-2-(trifluoromethyl)imidazole (LiTDI), can delay the degradation reaction as well as improve the cycling stability of LiNi1/3Mn1/3Co1/3O2/Li metal batteries at 55 degrees C. This work highlights the poor shelf life of electrolytes containing FEC in combination with LiPF6 and thereby the great importance of developing proper storage methods as well as optimizing the content of FEC in practical cells.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 2, no 7, p. 4925-4935
Keywords [en]
lithium metal batteries, thermal instability, electrolyte storage instability, fluoroethylene carbonate, moisture scavenger, lithium 4, 5-dicyano-2-(trifluoromethyl)imidazole (LiTDI)
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-391950DOI: 10.1021/acsaem.9b00607ISI: 000477074700040OAI: oai:DiVA.org:uu-391950DiVA, id: diva2:1346768
Funder
Swedish Energy Agency, 40466-1Swedish Energy Agency, 39043-1EU, Horizon 2020, 685716Available from: 2019-08-29 Created: 2019-08-29 Last updated: 2019-08-29Bibliographically approved

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Xu, ChaoHernández, GuiomarEdström, KristinaBrandell, DanielMindemark, Jonas

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